CN116492978B - Zn 2+ Modified industryZAS/GRM composite material of waste red mud, and preparation method and application thereof - Google Patents
Zn 2+ Modified industryZAS/GRM composite material of waste red mud, and preparation method and application thereof Download PDFInfo
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- 239000002131 composite material Substances 0.000 title claims abstract description 41
- 238000002360 preparation method Methods 0.000 title claims abstract description 32
- 239000002699 waste material Substances 0.000 title abstract description 6
- 239000011701 zinc Substances 0.000 claims abstract description 67
- 239000003463 adsorbent Substances 0.000 claims abstract description 58
- 239000002440 industrial waste Substances 0.000 claims abstract description 43
- IQFVPQOLBLOTPF-HKXUKFGYSA-L congo red Chemical compound [Na+].[Na+].C1=CC=CC2=C(N)C(/N=N/C3=CC=C(C=C3)C3=CC=C(C=C3)/N=N/C3=C(C4=CC=CC=C4C(=C3)S([O-])(=O)=O)N)=CC(S([O-])(=O)=O)=C21 IQFVPQOLBLOTPF-HKXUKFGYSA-L 0.000 claims abstract description 19
- 238000000034 method Methods 0.000 claims abstract description 19
- 230000008569 process Effects 0.000 claims abstract description 10
- 229910000611 Zinc aluminium Inorganic materials 0.000 claims abstract description 7
- HXFVOUUOTHJFPX-UHFFFAOYSA-N alumane;zinc Chemical compound [AlH3].[Zn] HXFVOUUOTHJFPX-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000002351 wastewater Substances 0.000 claims abstract description 7
- 239000002245 particle Substances 0.000 claims description 37
- 239000010881 fly ash Substances 0.000 claims description 26
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 15
- 238000001035 drying Methods 0.000 claims description 12
- 238000003756 stirring Methods 0.000 claims description 12
- 229910052725 zinc Inorganic materials 0.000 claims description 11
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 10
- 238000001914 filtration Methods 0.000 claims description 10
- 238000002156 mixing Methods 0.000 claims description 10
- 238000005469 granulation Methods 0.000 claims description 6
- 230000003179 granulation Effects 0.000 claims description 6
- 239000000853 adhesive Substances 0.000 claims description 5
- 230000001070 adhesive effect Effects 0.000 claims description 5
- 238000007605 air drying Methods 0.000 claims description 5
- 239000003795 chemical substances by application Substances 0.000 claims description 5
- 239000002957 persistent organic pollutant Substances 0.000 claims description 5
- 229910045601 alloy Inorganic materials 0.000 claims description 3
- 239000000956 alloy Substances 0.000 claims description 3
- 238000001179 sorption measurement Methods 0.000 abstract description 31
- 239000000463 material Substances 0.000 abstract description 15
- 229910001385 heavy metal Inorganic materials 0.000 abstract description 12
- 238000004519 manufacturing process Methods 0.000 abstract description 7
- 239000002994 raw material Substances 0.000 abstract description 3
- 230000015572 biosynthetic process Effects 0.000 abstract description 2
- 238000003786 synthesis reaction Methods 0.000 abstract description 2
- 238000007598 dipping method Methods 0.000 abstract 1
- 239000000843 powder Substances 0.000 description 16
- 239000000243 solution Substances 0.000 description 12
- 238000005342 ion exchange Methods 0.000 description 9
- 238000002474 experimental method Methods 0.000 description 8
- 239000011230 binding agent Substances 0.000 description 7
- 239000008367 deionised water Substances 0.000 description 7
- 229910021641 deionized water Inorganic materials 0.000 description 7
- 239000007858 starting material Substances 0.000 description 7
- 230000000694 effects Effects 0.000 description 5
- 230000004048 modification Effects 0.000 description 5
- 238000012986 modification Methods 0.000 description 5
- 239000011148 porous material Substances 0.000 description 5
- 239000011734 sodium Substances 0.000 description 5
- 150000003751 zinc Chemical class 0.000 description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 4
- 238000007385 chemical modification Methods 0.000 description 4
- 239000002105 nanoparticle Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 239000000356 contaminant Substances 0.000 description 3
- 238000005470 impregnation Methods 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 238000012512 characterization method Methods 0.000 description 2
- 239000003086 colorant Substances 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 125000000524 functional group Chemical group 0.000 description 2
- 231100001261 hazardous Toxicity 0.000 description 2
- 125000003010 ionic group Chemical group 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 238000002386 leaching Methods 0.000 description 2
- 230000007246 mechanism Effects 0.000 description 2
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical group O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 229910052814 silicon oxide Inorganic materials 0.000 description 2
- 239000004094 surface-active agent Substances 0.000 description 2
- 229910018557 Si O Inorganic materials 0.000 description 1
- 239000004115 Sodium Silicate Substances 0.000 description 1
- 229920002472 Starch Polymers 0.000 description 1
- PTFCDOFLOPIGGS-UHFFFAOYSA-N Zinc dication Chemical compound [Zn+2] PTFCDOFLOPIGGS-UHFFFAOYSA-N 0.000 description 1
- 239000004480 active ingredient Substances 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- 239000000440 bentonite Substances 0.000 description 1
- 229910000278 bentonite Inorganic materials 0.000 description 1
- SVPXDRXYRYOSEX-UHFFFAOYSA-N bentoquatam Chemical compound O.O=[Si]=O.O=[Al]O[Al]=O SVPXDRXYRYOSEX-UHFFFAOYSA-N 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000009881 electrostatic interaction Effects 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 238000003933 environmental pollution control Methods 0.000 description 1
- 230000014509 gene expression Effects 0.000 description 1
- 239000003673 groundwater Substances 0.000 description 1
- 238000000024 high-resolution transmission electron micrograph Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 230000001850 reproductive effect Effects 0.000 description 1
- 230000000241 respiratory effect Effects 0.000 description 1
- 239000012266 salt solution Substances 0.000 description 1
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Inorganic materials [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 1
- 229910000029 sodium carbonate Inorganic materials 0.000 description 1
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 description 1
- 229910052911 sodium silicate Inorganic materials 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 239000002910 solid waste Substances 0.000 description 1
- 238000002336 sorption--desorption measurement Methods 0.000 description 1
- 239000008107 starch Substances 0.000 description 1
- 235000019698 starch Nutrition 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 238000003911 water pollution Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/0203—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising compounds of metals not provided for in B01J20/04
- B01J20/024—Compounds of Zn, Cd, Hg
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/04—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising compounds of alkali metals, alkaline earth metals or magnesium
- B01J20/043—Carbonates or bicarbonates, e.g. limestone, dolomite, aragonite
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/12—Naturally occurring clays or bleaching earth
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/16—Alumino-silicates
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
- B01J20/24—Naturally occurring macromolecular compounds, e.g. humic acids or their derivatives
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/281—Treatment of water, waste water, or sewage by sorption using inorganic sorbents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/286—Treatment of water, waste water, or sewage by sorption using natural organic sorbents or derivatives thereof
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2220/00—Aspects relating to sorbent materials
- B01J2220/40—Aspects relating to the composition of sorbent or filter aid materials
- B01J2220/48—Sorbents characterised by the starting material used for their preparation
- B01J2220/4875—Sorbents characterised by the starting material used for their preparation the starting material being a waste, residue or of undefined composition
- B01J2220/4887—Residues, wastes, e.g. garbage, municipal or industrial sludges, compost, animal manure; fly-ashes
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Analytical Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Geochemistry & Mineralogy (AREA)
- Dispersion Chemistry (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
- Water Treatment By Sorption (AREA)
Abstract
The invention discloses a Zn 2+ ZAS/GRM composite material of modified industrial waste red mud, a preparation method and application thereof, and belongs to the technical field of adsorbent preparation. The method takes the industrial waste red mud as the raw material, and prepares Zn by utilizing the dipping and baking processes which are simple, efficient and capable of mass production 2+ Nano zinc aluminum silicate/granular red mud (ZAS/GRM) adsorbent of modified red mud; the synthesis process of the material is simple and easy to operate; in addition, nano Zinc Aluminum Silicate (ZAS) on the outer layer of Granular Red Mud (GRM) can effectively prevent the leakage of heavy metal elements in the GRM, and solves the problems of difficult treatment and utilization of the red mud and heavy metal pollution in industry. The ZAS layer is used for improving the adsorption capacity of the composite material to Congo Red (CR) dye wastewater, and is also used as a shell for effectively encapsulating heavy metal elements in GRM. The purpose of treating dye wastewater with waste is achieved by adopting industrial waste, and a new idea is provided for industrial application of red mud.
Description
Technical Field
The invention belongs to the technical field of adsorbent preparation, and in particular relates to Zn 2+ ZAS/GRM composite material of modified industrial waste red mud, and a preparation method and application thereof.
Background
Congo Red (CR) is a typical organic dye contaminant with high stability and non-degradability. CR is extremely difficult to remove from wastewater due to its water solubility and high stability. Furthermore, CR has been shown to be toxic and carcinogenic to biological systems, including respiratory, reproductive, ocular and skin systems. The detection of CR in water has attracted public attention and there is an urgent need to develop a viable and effective strategy to mitigate its impact on the aqueous environment. Adsorption has proven to be a technique that can effectively remove CR. Because of low cost and convenient treatment, the adsorption method is widely applied to actual production. In general, there are three basic types of adsorption methods, including physical adsorption, chemical adsorption, and electrostatic interaction adsorption. Furthermore, the selection of the appropriate type of adsorbent is critical to efficient CR removal.
Red Mud (RM) is a solid waste produced in the alumina production process. RM is generally considered a hazardous contaminant due to its strong basicity and its containing a list of hazardous heavy metal elements, etc. It is counted that production of alumina per ton inevitably leads to emissions of 1-2 tons RM. China is a large country for alumina production, the annual production of RM is about 5000 ten thousand tons, and the total stock of RM in China is up to 5 hundred million tons at present. Typically, alumina factories mostly transport RM to storage yards for stockpiling in the form of open air damming. However, the large-scale stockpiling of RM can cause serious pollution to soil and groundwater resources in the surrounding area due to the strong alkalinity of RM and the bad characteristics of heavy metals. Therefore, reducing the pollution of the RM to the environment and realizing the resource utilization of the RM are important technical difficulties.
The original RM is in powder shape, has an average particle diameter of about 3-10 mu m and a large specific surface area, and can be used as a dye adsorption material. However, if the original powdery RM is directly adopted for adsorption, the adsorption capacity of the RM to pollutants is limited, and heavy metal elements are leached out in the adsorption process, so that secondary pollution of water is caused. In addition, the original powdery RM is not easy to recycle and reuse, and the cost of large-scale application is high and the reproducibility is poor. Currently, the "granulation" of powdered RM has become a trend in RM research. In general, bentonite, fly ash, starch, sodium carbonate, sodium silicate and other substances are added into RM to prepare the RM into large-particle red mud (GRM), and the GRM is more beneficial to actual production and industrial application.
GRM is used as dye adsorbent and has excellent CR adsorbing capacity. In addition, GRM also shows the potential to improve its adsorption properties by altering its surface activity. The physical and chemical modification methods can improve the adsorption performance of the GRM. Compared with physical modification, chemical modification can directly change the surface chemical property of GRM by introducing specific functional groups or surfactants, thereby improving the surface performance and adsorption capacity of GRM. In addition, by introducing appropriate functional groups or surfactants through chemical modification, the interaction between the GRM and the adsorbed molecules can be selectively enhanced, thereby improving the stability and the service life of the GRM. Ion exchange has proven to be an effective modification as a chemical modification. The surface charge amount of the GRM is significantly increased by substituting the ionic group on the surface of the GRM, thereby enhancing the adsorption capability between the GRM and the organic dye. In addition, the ion exchange method can change the pore diameter and the porosity of GRM and improve the specific surface area and the adsorption efficiency. However, the ion exchange method is not widely used due to high cost and low selectivity limitations. Therefore, the selection of suitable ionic groups for surface ion exchange with GRM is critical to enhance its adsorption properties.
Zinc salts are chosen as suitable materials for surface ion exchange with GRM, mainly because of the following advantages: 1) Zinc salt is used as a chemical substance widely existing in the nature and is a high cost performance choice for large-scale application; 2) The ion exchange of the zinc salt increases the surface charge quantity of the GRM, thereby improving the adsorption capacity of the GRM to organic dye; 3) By regulating and controlling the concentration of the zinc salt solution, the selective adsorption of GRM to specific pollutants can be realized. Typical nano Zinc Aluminum Silicate (ZAS) materials in zinc salts share an oxygen atom with each silicon oxide tetrahedron and adjacent aluminum oxide hexahedron in their crystal structure to form a T-O-T structure (where T represents a silicon oxide tetrahedron or aluminum oxide hexahedron) and then form a stable three-dimensional zinc aluminum silicate network structure from this structure and zinc ions. However, because ZAS is in a powder state, it is difficult to remove it after use, which causes secondary pollution. In addition, the powdery adsorbent has the defects of easy loss of active ingredients, difficult recovery, high large-scale application cost, poor reproducibility and the like, and severely limits the application of the powdery adsorbent in environmental pollution control.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide a Zn 2+ ZAS/GRM composite material of modified industrial waste red mud, and a preparation method and application thereof. Zn in ZAS is removed by a simple calcination process 2+ Na with GRM surface + Ion exchange is performed to firmly anchor ZAS to the surface of GRM, and ZAS/GRM adsorbents with high specific surface area can provide a large number of adsorption sites. In addition, the ZAS layer can prevent the leakage of heavy metal elements in GRM. The invention can solve the technical problems of difficult recovery, high cost for large-scale application, poor reproducibility and the like of the existing powdery red mud-based adsorbent, and solves the problem of secondary pollution of the red mud-based adsorbent to water.
In order to achieve the above purpose, the invention is realized by adopting the following technical scheme:
the invention discloses a Zn 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: adding red mud, fly ash, an adhesive and a pore-forming agent into water for mixing, then carrying out artificial granulation to obtain GRM, and then carrying out air drying and roasting on the GRM to obtain porous GRM particles;
s2: immersing porous GRM particles in a solution containing Zn 2+ Stirring the solution, filtering and drying to obtain ZAS/GRM adsorbent; roasting ZAS/GRM adsorbent to obtain Zn 2+ ZAS/GRM composite material of modified industrial waste red mud.
Further, in S1, the dosage ratio of the red mud, the fly ash, the adhesive, the pore-forming agent and the water is (70-80): (5-10): (5-15): (1-7): (20-200) mL;
the adhesive is C 6 H 12 O 6 The method comprises the steps of carrying out a first treatment on the surface of the The pore-forming agent is NaHCO 3 。
Further, in S1, the particle size of the GRM is 5-10 mm; the air drying time is 10-48 hours; the roasting process parameters are as follows: preheating for 0.1-2 h at 273-973K, and baking for 20-90 min at 873-1773K.
Further, in S2, the alloy contains Zn 2+ The solution is ZnCl 2 、ZnSO 4 Or ZnCO 3 A solution; the Zn-containing alloy comprises Zn 2+ The concentration of the solution is 0.10 to 0.30mol L -1 。
Further, in S2, the porous GRM particles and Zn-containing particles 2+ The dosage ratio of the solution is (1.0-15) g: (20-100) mL.
Further, in S2, stirring is continuously carried out for 10-48 hours at 200-900 rpm; the drying temperature is 273-600K.
Further, in S2, the process parameters of the baking treatment are as follows: baking at 600-973K for 1-5 h.
The invention also discloses Zn prepared by the preparation method 2+ ZAS/GRM composite material of modified industrial waste red mud.
The invention also discloses the Zn 2+ Application of ZAS/GRM composite material of modified industrial waste red mud, wherein Zn 2+ ZAS/GRM composite material of modified industrial waste red mudAn adsorbent for removing organic pollutants from wastewater.
Further, the organic contaminant is congo red.
Compared with the prior art, the invention has the following beneficial effects:
the invention discloses a Zn 2+ The preparation method of ZAS/GRM (nano zinc aluminum silicate/granular red mud) composite material of modified industrial waste red mud uses cheap red mud as raw material, and adopts simple, high-efficiency and large-scale production impregnation and baking process to prepare Zn 2+ ZAS/GRM adsorbent of modified industrial waste red mud (nano zinc aluminum silicate/granular red mud adsorbent); the synthesis process is simple and easy to operate; in addition, the ZAS layer on the outer layer can effectively prevent the leakage of heavy metal elements in the GRM, solves the problem of secondary pollution of the GRM in industry, improves the adsorption capacity of the ZAS/GRM by using the ZAS layer, and provides a new thought for treating waste with waste as a shell for packaging heavy metal elements in the GRM. The invention not only solves the problem of dye water pollution by utilizing the strategy of treating waste with waste, but also realizes the recycling utilization of industrial waste red mud.
The invention also discloses the Zn 2+ The ZAS/GRM composite material of the modified industrial waste red mud is applied to congo red removal, and the ZAS/GRM adsorbent greatly improves the removal efficiency of organic pollutant congo red in wastewater.
Drawings
FIG. 1 is a schematic diagram of ZnCl before and after GRM addition 2 Color comparison of the impregnating solution;
FIG. 2 is the leaching concentration of heavy metal ions for ZAS/GRM composite material of example 4;
FIG. 3 is a graph of pore size distribution curves for different materials;
wherein: a-ZAS/GRM composite of example 4; b-porous GRM particles and ZAS/GRM adsorbent;
FIG. 4 is a color comparison of ZAS/GRM composite material of example 4 before and after CR adsorption;
FIG. 5 is a comparison of the effect of porous GRM particles and ZAS/GRM adsorbent on CR removal in example 4;
FIG. 6 is a graph of characterization of ZAS nanoparticles on the surface of ZAS/GRM adsorbent in example 4;
wherein: a-transmission electron microscope photograph; b-high resolution transmission electron micrographs; c-ZAS/GRM.
Detailed Description
So that those skilled in the art can appreciate the features and effects of the present invention, a general description and definition of the terms and expressions set forth in the specification and claims follows. Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs, and in the event of a conflict, the present specification shall control.
The theory or mechanism described and disclosed herein, whether right or wrong, is not meant to limit the scope of the invention in any way, i.e., the present disclosure may be practiced without limitation to any particular theory or mechanism.
All features such as values, amounts, and concentrations that are defined herein in the numerical or percent ranges are for brevity and convenience only. Accordingly, the description of a numerical range or percentage range should be considered to cover and specifically disclose all possible sub-ranges and individual values (including integers and fractions) within the range.
Herein, unless otherwise indicated, "comprising," "including," "having," or similar terms encompass the meanings of "consisting of … …" and "consisting essentially of … …," e.g., "a includes a" encompasses the meanings of "a includes a and the other and" a includes a only.
In this context, not all possible combinations of the individual technical features in the individual embodiments or examples are described in order to simplify the description. Accordingly, as long as there is no contradiction between the combinations of these technical features, any combination of the technical features in the respective embodiments or examples is possible, and all possible combinations should be considered as being within the scope of the present specification.
As shown in FIG. 1, the present invention discloses a Zn 2+ The preparation method of ZAS/GRM composite material of modified industrial waste red mud comprisesThe method comprises the following steps:
s1: adding red mud, fly ash, an adhesive and a pore-forming agent into water for mixing, then carrying out artificial granulation to obtain GRM, and then carrying out air drying and roasting on the GRM to obtain porous GRM particles;
s2: immersing porous GRM particles in a solution containing Zn 2+ Stirring the solution, filtering and drying to obtain ZAS/GRM adsorbent; roasting ZAS/GRM adsorbent to obtain Zn 2+ ZAS/GRM composite material of modified industrial waste red mud.
The invention will be further illustrated with reference to specific examples. It is to be understood that these examples are illustrative of the present invention and are not intended to limit the scope of the present invention. Further, it is understood that various changes and modifications may be made by those skilled in the art after reading the teachings of the present invention, and such equivalents are intended to fall within the scope of the claims appended hereto.
The following examples use instrumentation conventional in the art. The experimental methods, in which specific conditions are not noted in the following examples, are generally conducted under conventional conditions or under conditions recommended by the manufacturer. The following examples used various starting materials, unless otherwise indicated, were conventional commercial products, the specifications of which are conventional in the art. In the description of the present invention and the following examples, "%" means weight percent, and "parts" means parts by weight, and ratios means weight ratio, unless otherwise specified.
Example 1
Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: red Mud (RM), fly Ash (FA), naHCO 3 And C 6 H 12 O 6 (binder) as a starting material, was thoroughly ground and screened through a 100 mesh sieve, then in RM: FA: naHCO (NaHCO) 3 ：C 6 H 12 O 6 Is 70:10:10: mixing the materials according to the mass ratio of 10 to obtain powder A; then adding 20mL of deionized water into the powder A to form a mud cake, and manually granulating to obtain GRM with the particle size of 5 mm; then, willAfter the GRM is air-dried for 24 hours, preheating for 0.1 hour at 273K, baking for 20 minutes at 873K, and finally preparing porous GRM particles;
s2: preparation of 20mL of 0.10mol L -1 ZnCl 2 Subsequently immersing 1g of porous GRM particles in ZnCl 2 Continuously stirring at 200rpm at the same time, after 10 hours, obtaining the ZAS/GRM adsorbent by filtration and drying at 273K; the ZAS/CRM adsorbent obtained was treated at 600K for 1h before the adsorption experiment to obtain a Zn 2+ Modified industrial waste red mud adsorbent.
Example 2
Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: red Mud (RM), fly Ash (FA), naHCO 3 And C 6 H 12 O 6 (binder) as a starting material, was thoroughly ground and screened through a 300 mesh sieve, then in RM: FA: naHCO (NaHCO) 3 ：C 6 H 12 O 6 Is 70:10:10: mixing the materials according to the mass ratio of 10 to obtain powder A; adding 200mL of deionized water into the powder A to form a mud cake, and manually granulating to obtain GRM with the particle size of 7 mm; then, after the GRM is air-dried for 10 hours, preheating for 1.5 hours at 573K, and baking for 20 minutes at 973K, and finally, preparing porous GRM particles;
s2: preparation of 50mL of 0.17mol L -1 ZnCl 2 Subsequently immersing 8g of porous GRM particles in ZnCl 2 Continuously stirring at 900rpm at the same time, after 48 hours, obtaining the ZAS/GRM adsorbent by filtration and drying at 273K; the ZAS/CRM adsorbent obtained was treated at 600K for 5h before the adsorption experiment to obtain a Zn 2+ Modified industrial waste red mud adsorbent.
Example 3
Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: red Mud (RM), fly Ash (FA), naHCO 3 And C 6 H 12 O 6 (binder) as raw material and passed through 100 meshScreens were screened and then run on RM: FA: naHCO (NaHCO) 3 ：C 6 H 12 O 6 Is 75:10:5: mixing the materials according to the mass ratio of 10 to obtain powder A; then adding 100mL of deionized water into the powder A to form a mud cake, and manually granulating to obtain GRM with the particle size of 6 mm; then, after the GRM is air-dried for 36 hours, preheating for 2 hours at 673K, and baking for 60 minutes at 1173K, and finally, preparing porous GRM particles;
s2: preparation of 80mL of 0.3mol L -1 ZnCl 2 Subsequently immersing 10g of porous GRM particles in ZnCl 2 Continuously stirring at 600rpm at the same time, after 48 hours, obtaining the ZAS/GRM adsorbent by filtration and drying at 500K; the ZAS/CRM adsorbent obtained was treated at 773K for 2.5h before the adsorption experiment to give a Zn 2+ Modified industrial waste red mud adsorbent.
Example 4
Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: red Mud (RM), fly Ash (FA), naHCO 3 And C 6 H 12 O 6 (binder) as a starting material, was thoroughly ground and screened through a 100 mesh sieve, then in RM: FA: naHCO (NaHCO) 3 ：C 6 H 12 O 6 Is 75:10:5: mixing the materials according to the mass ratio of 10 to obtain powder A; then adding 100mL of deionized water into the powder A to form a mud cake, and manually granulating to obtain GRM with the particle size of 7 mm; then, after the GRM is air-dried for 24 hours, preheating for 0.5 hour at 773K, baking for 20 minutes at 1173K, and finally preparing porous GRM particles;
s2: preparation of 150mL of 0.15mol L -1 ZnCl 2 Subsequently immersing 12g of porous GRM particles in ZnCl 2 Continuously stirring at 300rpm at the same time, after 24 hours, obtaining the ZAS/GRM adsorbent by filtration and drying at 333K; the ZAS/CRM adsorbent obtained was treated at 773K for 3h before the adsorption experiment to obtain a Zn 2+ Modified industrial waste red mud adsorbent.
Example 5
Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: red Mud (RM), fly Ash (FA), naHCO 3 And C 6 H 12 O 6 (binder) as a starting material, was thoroughly ground and screened through a 100 mesh sieve, then in RM: FA: naHCO (NaHCO) 3 ：C 6 H 12 O 6 Is 75:10:5: mixing the materials according to the mass ratio of 10 to obtain powder A; then 150mL of deionized water is added into the powder A to form a mud cake, and GRM with the particle size of 7mm is obtained through artificial granulation; then, after the GRM is air-dried for 42 hours, preheating for 1.5 hours at 773K, and baking for 50 minutes at 1073K, and finally, preparing porous GRM particles;
s2: preparation of 160mL of 0.25mol L -1 ZnCl 2 Subsequently immersing 13g of porous GRM particles in ZnCl 2 Continuously stirring at 800rpm for 48 hours, and filtering and drying at 600K to obtain ZAS/GRM adsorbent; the ZAS/CRM adsorbent obtained was treated at 873K for 5h before the adsorption experiment to obtain a Zn 2+ Modified industrial waste red mud adsorbent.
Example 6
Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: red Mud (RM), fly Ash (FA), naHCO 3 And C 6 H 12 O 6 (binder) as a starting material, was thoroughly ground and screened through a 100 mesh sieve, then in RM: FA: naHCO (NaHCO) 3 ：C 6 H 12 O 6 Is 75:10:5: mixing the materials according to the mass ratio of 10 to obtain powder A; then 180mL of deionized water is added into the powder A to form a mud cake, and GRM with the particle size of 6mm is obtained through artificial granulation; then, after the GRM is air-dried for 30 hours, preheating for 1 hour at 873K, and baking for 80 minutes at 973K, and finally, preparing porous GRM particles;
s2: preparation of 180mL of 0.15mol L -1 ZnCl 2 Is then immersed in ZnCl in 14g of porous GRM particles 2 While stirring continuously at 750rpm, for 40h, by filtration and drying at 573KObtaining the obtained ZAS/GRM adsorbent; the ZAS/CRM adsorbent obtained was treated at 673K for 4h before the adsorption experiment to obtain a Zn 2+ Modified industrial waste red mud adsorbent.
Example 7
Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud comprises the following steps:
s1: red Mud (RM), fly Ash (FA), naHCO 3 And C 6 H 12 O 6 (binder) as a starting material, was thoroughly ground and screened through a 300 mesh sieve, then in RM: FA: naHCO (NaHCO) 3 ：C 6 H 12 O 6 Is 80:5:5: mixing the materials according to the mass ratio of 10 to obtain powder A; adding 200mL of deionized water into the powder A to form a mud cake, and manually granulating to obtain GRM with the particle size of 7 mm; then, after the GRM is air-dried for 48 hours, preheating for 2 hours at 973K, and baking for 90 minutes at 1773K, and finally, preparing porous GRM particles;
s2: preparation of 200mL of 0.3mol L -1 ZnCl 2 Subsequently immersing 15g of porous GRM particles in ZnCl 2 Continuously stirring at 900rpm at the same time, after 48 hours, obtaining the ZAS/GRM adsorbent by filtration and drying at 600K; the ZAS/CRM adsorbent obtained was treated at 973K for 5h before the adsorption experiment to obtain a Zn 2+ Modified industrial waste red mud adsorbent.
FIG. 1 shows ZnCl before and after GRM addition 2 Comparison of the colors of the impregnating solutions, it can be seen from the figures that ZnCl is present after 24 hours of impregnation of the GRM 2 The impregnating solution changed from milky to pale yellow. Indicating Zn 2+ And Na (Na) + Ion exchange reactions occur during the impregnation process.
FIG. 2 shows the leaching concentration of heavy metal ions in the ZAS/GRM composite material of example 4, from which it can be seen that the concentration of heavy metal elements As, cd and Pb in the impregnating solution is below the wastewater discharge standard. In addition, with 0mol L -1 ZnCl 2 (aq) compared with 0.10, 0.15 and 0.20mol L -2 ZnCl 2 Na of (a) + The content increases sharply, indicating ZnCl 2 Zn of (2) 2+ And Na of GRM + Ion exchange occurs therebetween.
FIG. 3a is N of different materials 2 The adsorption-desorption curves show a distinct hysteresis loop of H3 type, indicating that GRM and ZAS/GRM adsorbents have mesoporous properties. Zn (zinc) 2+ After modification, the specific surface area of the porous ZAS/GRM adsorbent is 2.8911m 2 g -1 To 12.0333m 2 g -1 . The ZAS/GRM adsorbent with the specific surface area increased by 6 times provides more active sites for organic pollutants, thereby greatly improving the adsorption behavior. FIG. 3b further characterizes the mesoporous distribution of GRM and ZAS/GRM adsorbents. The mean pore size of the ZAS/GRM adsorbent was 25.412nm, while the mean pore size of the GRM adsorbent material was 41.918nm. The decrease in pore size is due to the loading of the ZAS nanoparticles on the GRM surface.
FIG. 4 is a comparison of colors before and after adsorption of CR by the ZAS/GRM composite material of example 4, from which it can be seen that CR is well adsorbed on the ZAS/GRM composite material, achieving a purification effect.
Fig. 5 is a comparison of the CR removal effect of the porous GRM particles and ZAS/GRM adsorbent of example 4, and it can be seen from the figure that the ZAS/GRM adsorbent can achieve efficient solid-liquid separation, thereby significantly reducing the loss of adsorbent quality and secondary pollution to the environment during the separation process.
FIG. 6 is a graph showing the performance characterization of ZAS nanoparticles on the surface of the ZAS/GRM adsorbent in example 4, and it can be seen from FIGS. 6a to 6c that the ZAS nanoparticles are uniformly distributed on the surface of the ZAS/GRM adsorbent, and the analysis result of the energy spectrometer shows that Zn, al, si and O elements are uniformly distributed on the surface of the ZAS/GRM adsorbent, indicating that Zn-Al-Si-O material is successfully formed on the surface of the GRM.
The above is only for illustrating the technical idea of the present invention, and the protection scope of the present invention is not limited by this, and any modification made on the basis of the technical scheme according to the technical idea of the present invention falls within the protection scope of the claims of the present invention.
Claims (9)
1. Zn (zinc) 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud is characterized by comprising the following steps of:
s1: adding red mud, fly ash, an adhesive and a pore-forming agent into water for mixing, then carrying out artificial granulation to obtain GRM, and then carrying out air drying and roasting on the GRM to obtain porous GRM particles;
s2: immersing porous GRM particles in a solution containing Zn 2+ Stirring the solution, and then filtering and drying to obtain a nano zinc aluminum silicate/granular red mud adsorbent, namely a ZAS/GRM adsorbent; roasting ZAS/GRM adsorbent to obtain Zn 2+ ZAS/GRM composite material of modified industrial waste red mud.
2. A Zn according to claim 1 2+ A preparation method of ZAS/GRM composite material of modified industrial waste red mud is characterized in that in S1, the particle size of GRM is 5-10 mm; the air drying time is 10-48 h; the roasting process parameters are as follows: preheating for 0.1-2 h at 573-973K, and baking for 20-90 min at 873-1773K.
3. A Zn according to claim 1 2+ A preparation method of ZAS/GRM composite material of modified industrial waste red mud is characterized in that in S2, the composite material contains Zn 2+ The solution is ZnCl 2 、ZnSO 4 Or ZnCO 3 A solution; the Zn-containing alloy comprises Zn 2+ The concentration of the solution is 0.10-0.30 mol L -1 。
4. A Zn according to claim 1 2+ A preparation method of ZAS/GRM composite material of modified industrial waste red mud is characterized in that in S2, the porous GRM particles and Zn are contained 2+ The dosage ratio of the solution is (1.0-15) g: (20-100) mL.
5. A Zn according to claim 1 2+ A preparation method of ZAS/GRM composite material of modified industrial waste red mud is characterized in that in S2, stirring is continuously carried out for 10-48 h at 200-900 rpm; the drying temperature is 333-600K.
6.A Zn according to claim 1 2+ The preparation method of the ZAS/GRM composite material of the modified industrial waste red mud is characterized in that in S2, the technological parameters of the roasting treatment are as follows: baking at 673-973K for 1-5 h.
7. Zn (zinc) 2+ ZAS/GRM composite material of modified industrial waste red mud, characterized in that a Zn as claimed in any one of claims 1 to 6 is used 2+ The ZAS/GRM composite material of the modified industrial waste red mud is prepared by a preparation method.
8. A Zn according to claim 7 2+ Application of ZAS/GRM composite material of modified industrial waste red mud is characterized in that the Zn 2+ ZAS/GRM composite material of modified industrial waste red mud is used as adsorbent for removing organic pollutant in waste water.
9. A Zn according to claim 8 2+ The application of the ZAS/GRM composite material of the modified industrial waste red mud is characterized in that the organic pollutant is Congo red.
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